Coupling Ni Single Atomic Sites with Metallic Aggregates at Adjacent Geometry on Carbon Support for Efficient Hydrogen Peroxide Electrosynthesis

© 2024 The Authors. Advanced Science published by Wiley‐VCH GmbH..

Single atomic catalysts have shown great potential in efficiently electro-converting O2 to H2O2 with high selectivity. However, the impact of coordination environment and introduction of extra metallic aggregates on catalytic performance still remains unclear. Herein, first a series of carbon-based catalysts with embedded coupling Ni single atomic sites and corresponding metallic nanoparticles at adjacent geometry is synthesized. Careful performance evaluation reveals NiSA/NiNP-NSCNT catalyst with precisely controlled active centers of synergetic adjacent Ni-N4S single sites and crystalline Ni nanoparticles exhibits a high H2O2 selectivity over 92.7% within a wide potential range (maximum selectivity can reach 98.4%). Theoretical studies uncover that spatially coupling single atomic NiN4S sites with metallic Ni aggregates in close proximity can optimize the adsorption behavior of key intermediates *OOH to achieve a nearly ideal binding strength, which thus affording a kinetically favorable pathway for H2O2 production. This strategy of manipulating the interaction between single atoms and metallic aggregates offers a promising direction to design new high-performance catalysts for practical H2O2 electrosynthesis.

Medienart:

E-Artikel

Erscheinungsjahr:

2024

Erschienen:

2024

Enthalten in:

Zur Gesamtaufnahme - year:2024

Enthalten in:

Advanced science (Weinheim, Baden-Wurttemberg, Germany) - (2024) vom: 11. Apr., Seite e2402240

Sprache:

Englisch

Beteiligte Personen:

Wang, Xin [VerfasserIn]
Huang, Run [VerfasserIn]
Mao, Xin [VerfasserIn]
Liu, Tian [VerfasserIn]
Guo, Panjie [VerfasserIn]
Sun, Hai [VerfasserIn]
Mao, Zhelin [VerfasserIn]
Han, Chao [VerfasserIn]
Zheng, Yarong [VerfasserIn]
Du, Aijun [VerfasserIn]
Liu, Jianwei [VerfasserIn]
Jia, Yi [VerfasserIn]
Wang, Lei [VerfasserIn]

Links:

Volltext

Themen:

Heteroatom doped carbon matrix
Hydrogen peroxide electrosynthesis
Journal Article
Nanoparticles
Single atoms
Synergistic effect

Anmerkungen:

Date Revised 12.04.2024

published: Print-Electronic

Citation Status Publisher

doi:

10.1002/advs.202402240

funding:

Förderinstitution / Projekttitel:

PPN (Katalog-ID):

NLM370949161